Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands

The 5-HT2AR is a target in neuropsychiatric conditions such as psychosis, which is commonly managed with atypical antipsychotics. These have associated side effects due to off-target interactions. Consequently, there is a demand to develop therapeutics that exhibit no affinity for these off-target s...

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Main Author: Damerum, Luke
Format: Thesis (University of Nottingham only)
Language:English
Published: 2024
Subjects:
Online Access:https://eprints.nottingham.ac.uk/78719/
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author Damerum, Luke
author_facet Damerum, Luke
author_sort Damerum, Luke
building Nottingham Research Data Repository
collection Online Access
description The 5-HT2AR is a target in neuropsychiatric conditions such as psychosis, which is commonly managed with atypical antipsychotics. These have associated side effects due to off-target interactions. Consequently, there is a demand to develop therapeutics that exhibit no affinity for these off-target sites. Moreover, in recent 5-HT2AR X-ray crystal structures, a unique hydrophobic pocket or passage between transmembrane helices 4 and 5 sets it apart from other 5-HT2 receptor subtypes. This structural feature is implicated in the selectivity demonstrated by therapeutic pimavanserin towards the 5-HT2AR, owing to its binding conformation. Thus, presenting it as a target to interrogate for enhancing 5-HT2AR binding. A structure-based approach was used to design a pimavanserin analogue series targeting transmembrane helices 4 and 5. In silico studies involving docking and MM-GBSA calculations using a 5-HT2AR homology model (RMSD 0.09 Å) predicted several analogues to demonstrate improved binding compared to pimavanserin. Synthesis of the series yielded low to moderate yields. To evaluate the binding of the series experimentally a cell membrane-based fluorescent time-resolved Förster resonance energy transfer (TR-FRET) methodology was chosen. This led to the development of a high-affinity 5-HT2AR fluorescent probe, and determination of kinetic rates, (Kd 1.74 ± 0.46 nM, Kon 1.96 ± 0.13 x 108 M−1 min−1, and Koff 0.42 ± 0.02 min−1) characterised at SNAP-tagged human 5-HT2AR expressed in Chinese hamster ovary membranes.
first_indexed 2025-11-14T21:02:04Z
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institution University of Nottingham Malaysia Campus
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language English
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publishDate 2024
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spelling nottingham-787192024-12-13T04:40:08Z https://eprints.nottingham.ac.uk/78719/ Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands Damerum, Luke The 5-HT2AR is a target in neuropsychiatric conditions such as psychosis, which is commonly managed with atypical antipsychotics. These have associated side effects due to off-target interactions. Consequently, there is a demand to develop therapeutics that exhibit no affinity for these off-target sites. Moreover, in recent 5-HT2AR X-ray crystal structures, a unique hydrophobic pocket or passage between transmembrane helices 4 and 5 sets it apart from other 5-HT2 receptor subtypes. This structural feature is implicated in the selectivity demonstrated by therapeutic pimavanserin towards the 5-HT2AR, owing to its binding conformation. Thus, presenting it as a target to interrogate for enhancing 5-HT2AR binding. A structure-based approach was used to design a pimavanserin analogue series targeting transmembrane helices 4 and 5. In silico studies involving docking and MM-GBSA calculations using a 5-HT2AR homology model (RMSD 0.09 Å) predicted several analogues to demonstrate improved binding compared to pimavanserin. Synthesis of the series yielded low to moderate yields. To evaluate the binding of the series experimentally a cell membrane-based fluorescent time-resolved Förster resonance energy transfer (TR-FRET) methodology was chosen. This led to the development of a high-affinity 5-HT2AR fluorescent probe, and determination of kinetic rates, (Kd 1.74 ± 0.46 nM, Kon 1.96 ± 0.13 x 108 M−1 min−1, and Koff 0.42 ± 0.02 min−1) characterised at SNAP-tagged human 5-HT2AR expressed in Chinese hamster ovary membranes. 2024-12-13 Thesis (University of Nottingham only) NonPeerReviewed application/pdf en cc_by https://eprints.nottingham.ac.uk/78719/1/L_Damerum%20thesis%20Chemical%20and%20in%20silico%20exploration%20of%20novel%205-hydroxytryptamine%202A%20receptor%205-HT2AR%20ligands%20final_corrected_V1.pdf Damerum, Luke (2024) Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands. PhD thesis, University of Nottingham. 5-HT2A serotonin 2A receptor GPCR structure based drug design membrane proteins
spellingShingle 5-HT2A
serotonin 2A receptor
GPCR
structure based drug design
membrane proteins
Damerum, Luke
Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands
title Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands
title_full Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands
title_fullStr Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands
title_full_unstemmed Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands
title_short Chemical and in silico exploration of novel 5-hydroxytryptamine 2A receptor (5-HT2AR) ligands
title_sort chemical and in silico exploration of novel 5-hydroxytryptamine 2a receptor (5-ht2ar) ligands
topic 5-HT2A
serotonin 2A receptor
GPCR
structure based drug design
membrane proteins
url https://eprints.nottingham.ac.uk/78719/